Modeling and Simulation of Plasma-Assisted Ignition and Combustion

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1 Modeling and Simulation of Plasma-Assisted Ignition and Combustion Vigor Yang and Sharath Nagaraja Georgia Institute of Technology Atlanta, GA AFOSR MURI Fundamental Mechanisms, Predictive Modeling, and Novel Aerospace Applications of Plasma Assisted Combustion

2 Summary of Progress Plasma Flow Reactor Air Plasma self-consistent simulations of pulsed nanosecond discharges in air. detailed validation with experiments and analytical model results. demonstration of volumetric plasma heating and radical production of critical importance in combustion applications. Ignition of H -, CH 4 -, and C H 4 -Air Mixtures critical assessment of plasma kinetic models through comparison of OH decay rates after a burst of nanosecond pulses below ignition threshold temperatures (~500 K). importance of local plasma chemistry effects over heat transport in achieving volumetric ignition using pulse nanosecond discharges. detailed parametric studies on the sensitivity of nanosecond plasma ignition to pressure, eq. ratio, pulsing frequency, burst size, initial temperature, and dielectric properties. Ignition of Heavy Fuels (n-heptane) effect of nanosecond plasma on the two-stage n-heptane ignition process. Plasma-Coupled Premixed Flames construction of plasma flame kinetic mechanisms, including electron impact dynamics of all major species in flame environments (both reactants and products). effect of species and temperature gradients in the flame zone on the spatial characteristics of the plasma (E/N, electron density etc.) focus on plasma radical generation in the preheat zone and the impact on overall flame characteristics.

3 Publications 1. S. Nagaraja, V. Yang, I. Adamovich, Multi-Scale Modeling of Pulsed Nanosecond Dielectric Barrier Discharges in Plane-to-Plane Geometry, Journal of Physics D: Applied Physics 46 (15), 013, S. Nagaraja, V. Yang, Z. Yin and I. Adamovich, Ignition of Hydrogen-Air Mixtures using Pulsed Nanosecond Dielectric Barrier Plasma Discharges in Plane-to-Plane Geometry, Combustion and Flame, 013, in press 3. S. Nagaraja, and V. Yang, Detailed Comparison between Nanosecond Plasma and Thermal Ignition of Hydrogen-Air Mixtures to be submitted to Combustion and Flame. 4. S. Nagaraja and V. Yang, Numerical Investigation of Nanosecond Plasma Assisted Ignition of H -, CH 4 - and C H 4 -Air Mixtures to be submitted to Combustion and Flame. 5. S. Nagaraja, W. Sun and V. Yang, Nanosecond Plasma Assisted Ignition of n-heptane- Air Mixtures, in preparation.

4 Plasma-Assisted Combustion Modeling Framework Model Assumptions Governing Equations Plasma fluid with drift-diffusion approximation. Two temperature model: electrons at T e (defined using mean energy); ions and neutrals at gas temperature, T gas Lookup table for electron transport and rates using two-term expansion for electron Boltzmann equation (BOLSIG). Solution to mean-energy equation to update electron coefficients at each time step. Uniform pre-ionization in the discharge volume. No photo-ionization source term. Continuity Momentum Energy Species Continuity Equation of State Electron Energy Electric Potential u i 0 t x u ( uu ) i p Fi t x x x [( p) u ] ( ui ij ) i q i Sg t x x x n t k n t i i j ij EHD j i j. J N 1 i 1 Electric Field E i i j k S p Y RT Y R T. J S ; n ne 0 k i i gas e e e.( ) e( n n n e ) Validity of the BOLSIG approach to calculate electron rate coefficients, among other assumptions, has been validated through comparison of species density (O and OH), temperature and input energy with experiments

5 Nanosecond Plasma Assisted Ignition and Combustion Multi-Scale Modeling Framework PLASMA DISCHARGE DYNAMICS Plasma Chemistry Ionization, Excitation, Dissociation, Recombination FLOW AND COMBUSTION DYNAMICS Ignition and Combustion Chemistry Radical initiation, Chain propagation, termination, Fuel oxidation ns μs ms time ionization wave propagation electrical breakdown cathode sheath formation electron impact dynamics quenching of excited species ion recombination gas heating Solution Algorithm cumulative effects of multiple discharge pulses convective and diffusive transport ignition and combustion electric field Implicit LU decomposition electron energy Implicit GMRES electron and gas transport coefficients plasma species and flow conservation equations

6 Strategies for Computational Efficiency nanosecond voltage pulses time gap between voltage pulses Adaptive Time-Stepping Δt varies between s Semi-implicit treatment of the Poisson equation to circumvent the stiffness arising from tight coupling between electric field and electron density. Δt fixed at 10-9 s. Electron energy equation and Poisson equation are not solved since electric field effects become negligible and the space charge density rapidly decay as the applied voltage ends. Multi Time-Scale Treatment of Chemical Source Term speedup by 40% is seen by using the multi time-scale treatment of chemical source terms, but not orders of magnitude speedup observed in combustion simulations without plasma discharge. at high pulsing frequencies, the savings with using HMTS reduce because more time spent in simulating electric field transients during breakdown in each voltage pulse. * Gou et al., Combustion and Flame 157 (010)

7 Strategies for Computational Efficiency plasma combustion chemistry optimization charged species densities at center of discharge gap O, H and OH densities at center of discharge gap H -air ϕ = 1 94 torr 473 K 8 pulse burst full chem: 35 species, 87 reactions optimized chem: 19 species 111 reactions simulated a burst of 8 nanosec pulses with detailed mechanism. removed species with peak mole-fraction less than 10-8 ensured that E/N, electron and radical species densities and temperature (in both space and time, all within 10%) are accurately predicted by the reduced mechanism. provides a speed-up of ~ 4 times with H -air plasma ignition. expect greater savings with large C x H y mechanisms and D/3D simulations.

8 OSU Plasma Flow Reactor torr, K, khz ICCD images of discharge structure measurements time resolved O density using TALIF (uncertainty +/- 30%) time resolved NO density using LIF (uncertainty +/- 30%) time resolved OH density using LIF (uncertainty +/- 0%) time resolved temperature using rotational CARS and/or LIF thermometry ignition delay time from OH* emission rise ICCD imaging of discharge structure and flame kernel evolution. Front View ( cm 1 cm) Air : 373 K, 60 torr, 40 khz Side View (6 cm 1 cm) H - Air : 40 khz C H 4 - Air : 40 khz Pulse #0 Pulse #100 Pulse #00 67 torr, 300 K Pulse #00 50 torr, 300 K Pulse #400 Pulse #800 Pulse #00 84 torr, 373 K Pulse # torr, 473 K Pulse #00 60 torr, 373 K Pulse #00 84 torr, 473 K

9 cm Burner Facility Configurations OSU Plasma-Coupled Premixed Flat Flame direct coupled configuration low pressure 1D flame (0-30 torr) H /O /N, CH 4 /O /N and C H 4 /O /N premixed flames FID pulser: 14 kv peak voltage, 7 ns FWHM, ~3 mj/pulse Plasma off Plasma ON plasma upstream configuration Measurements spatially resolved OH density using LIF spatially resolved temperature using five-line OH thermometry. Plasma off Plasma ON

10 Nanosecond Pulsed Dielectric Plasma Simulations in N /Air Objectives Self-consistent simulations of pulsed nanosecond discharges in air with detailed kinetics. Validation with experiments and analytical model results. Direct insight into plasma heating and radical production of critical importance in combustion applications. Model Geometry Operating Conditions: Applied Waveform Initial Pressure: 60 torr Initial Temperature: 300 K Pulsing Frequency: 40 khz Gap width: 1 cm Initial Electron Density: 10 7 cm -3 Dielectric thickness: 1.75 mm Dielectric Constant: 4.3 Pulse Duration: 100 ns, FWHM: 1 ns Peak Voltage: -.5 kv and kv S. Nagaraja, V. Yang, I. Adamovich, Multi-Scale Modeling of Pulsed Nanosecond Dielectric Barrier Discharges in Plane-to-Plane Geometry, Journal of Physics D: Applied Physics 46 (15), 013,

11 Experimental Validation (Air Discharge) Coupled Pulse Energy O density at center of discharge volume coupled energy, temperature and O atom density predicted by the 1D model are within 0, 5 and 10% of experimental data, respectively. coupled energy remains fairly constant with pulse number, increasing linearly with pressure, and nearly independent of pulsing rates. O atom production via electron impact dissociation and quenching of excited N by O is captured accurately along with subsequent decay via formation of O 3 over ms timescales.

12 Detailed Physics over ns-ms Timescales air discharge (60 torr, 300 K, 40 khz, 100 pulses) temperature evolution for 100 nanosecond pulses spatial distribution of O atom density for 100 nanosecond pulses plasma heating effect is about 0.5-1K/pulse in air and nearly independent of pulsing frequency (as a function of pulse number). rapid gas heating produces weak acoustic waves which propagate into the gas volume from both ends. The strength of these waves becomes weak as overall temperature rises from heat release from quenching of excited species. a fairly uniform temperature profile develops in the plasma volume after several discharge pulses, owing to slow but steady (~0.5 K/pulse) heat release primarily from relaxation of excited species. repetitive pulsing results in efficient production of atomic oxygen through electron impact dissociation during discharge pulses, and quenching of excited nitrogen species by oxygen. volumetric radical generation and heating by pulsed discharges are of great significance for ignition and flame stabilization purposes.

13 Nanosecond Pulsed Dielectric Plasma in H -Air Mixtures model geometry operating conditions applied waveforms Pressure: torr Temperature: K Pulsing Frequency: khz Gap width: 1 cm Initial Electron Density: 10 7 cm -3 Dielectric thickness (Quartz): 1.75 mm Dielectric thickness (Kalrez): 1.58 mm Dielectric Constant (Quartz): 4.3 Dielectric Constant (Kalrez): 4-9 voltage and current Objectives comparison of OH density with measurements after a burst of 50 pulses. assess the accuracy of kinetics model at low temperature, pre-ignition conditions detailed investigations of NS plasma ignition physics and chemistry. sensitivity of ignition process to key system parameters and material properties. S. Nagaraja, V. Yang, Z. Yin and I. Adamovich, Ignition of Hydrogen-Air Mixtures using Pulsed Nanosecond Dielectric Barrier Plasma Discharges in Plane-to-Plane Geometry, Combustion and Flame (accepted).

14 H -Air Plasma Combustion Kinetics H /O /N Combustion Popov (008) + Konnov (008) for NOX chemistry chain initiation H O HO H H O OH OH H M H H M chain branching HO H OH OH HO H H O O HO O O OH H OH H O H O H O OH OH H O O OH O OH H O O H H OH H OH O H three body reactions H O M HO M O H M OH M O OH M H O M H H M H M O O M O M NOX reactions N O N NO N O NO O NO HO NO OH H /N /O Plasma dissociation/excitation ionic reactions quenching of excited species 4 N e N( S) N( D) e N e N A B C a e (,,, ) O e O O e H e H H e N e N e e N H HN H HN H O H O N 3 H O e H O H 3 N ( A ) O N O O 3 N ( B ) H N ( A ) H 3 3 N ( a ) H N H H 1 N( D) O O( D) NO 1 N A O N NO 3 ( ) 1 O( D) H OH H nonequilibrium plasma chemistry low temperature radical chemistry high temperature combustion chemistry low temperature ( K) uncertainties in many key chain branching reactions. detailed chemistry mechanism has 35 species and 87 reactions. reduced chemistry mechanism has 19 species and 111 reactions.

15 E/N and Electron Density Evolution P i = 80 torr, T i = 500 K, f = 60 khz, Φ = 1.0, FID Pulser E/N at center (60 pulses) E/N at center and input energy (first pulse) periodic steady-state peak value ~370 Td electron density at center (60 pulses) periodic steady-state peak value ~ 10 1 cm -3 breakdown voltage at these conditions occurs at ~10 kv sharp spike in current is seen at breakdown before it drops rapidly from the plasma shielding. plasma excited species production happens only during a short duration of ~5 ns when E/N is high. E/N and electron density reach a periodic steady state after ~8 pulses. nanosecond discharge efficiently generates radicals and excited species during each pulse because of high peak E/N.

16 Decay Rates of O, H and OH after a 50 pulse burst in H -air P i = 100 torr, T i = 500 K, f = 10 khz, FID pulser OH density at center of discharge gap O and H density at center of discharge gap key low temperature pathways for consumption of O and recirculation of H and OH H O M HO M O HO OH O H HO OH OH OH O H O model predictions for OH are within 10% of measurements in H -air mixtures, including both peak value and decay rates. O production is highly sensitive to changes in eq. ratio, increasing by ~50% when ϕ is decreased from 0.1 to H and OH are relatively insensitive, changing by ~10 % when eq. ratio is doubled.

17 How is ignition achieved with nanosecond plasma? P i = 80 torr, T i = 500 K, f = 60 khz, Φ = 1.0, FID pulser, 115 pulses ~ ms temperature evolution vs time spatial evolution of OH and temperature nearly nearly simultaneous simultaneous ignition ignition at different locations nanosecond plasma pulses creates a pool of O, H, and OH radicals (linear heating regime) increases temperature to a threshold value of ~700 K (nonlinear heating regime) partial fuel oxidation is triggered ignition and complete fuel oxidation heat transport plays a minor role. local plasma chemistry effects are critical in producing volumetric ignition secondary peaks in OH density near the boundaries is generated from HO which has accumulated due to low temperatures

18 Spatial Evolution of Radicals during H -Air Ignition P i = 80 torr, T i = 500 K, f = 60 khz, Φ = 1.0, FID pulser, 115 pulses ~ ms O H OH HO a small increase in temperature near ignition significantly increases the chain branching reaction rates. radical concentration profiles are much steeper than the temperature distribution, with well pronounced maxima near the centerline. both O and H densities increase by ~3 times within 0.4 ms near ignition, with OH density increasing by 4 times. low temperatures at the boundaries because of heat losses aid the accumulation of HO which generates OH. The secondary peaks in OH profiles near the boundaries result from this pathway.

19 H -air pulsed nanosecond plasma ignition what can we infer from emission images? OSU Experiment P i = 104 torr, T i = 473 K, f = 40 khz, Φ = 1.0, CPT pulser ignition first observed near edges, due to higher electric fields within 0.1 ms, ignition observed all along the centerline. the entire volume ignited within 0.4 ms of first detected flame emission. the present 1D model simulates a particular cross-section. although the 1D model cannot capture edge effects, it is able to explain the spreading of the ignition kernel from the centerline towards the boundaries. predictions are in line with observations that local plasma chemistry dominate over heat transport effects

20 Nanosecond Plasma Ignition vs Thermal Ignition is there any difference? species evolution at center for NS ignition ignition delay times with nanosecond plasma and a volume heat source P i = 80 torr T i = 500 K f = 60 khz Φ = 1.0 FID pulser 115 pulses N + e N (A 3, B 3,C 3 ) H + e H + H O + e O + O steps in the nanosecond plasma ignition process N (A 3 ) + O O + O(D) N (B 3,C 3 ) + H H + H O + OH H + O O + HO OH + O H + HO OH + OH H + OH H O + H the high activation energy chain initiation reactions are replaced by electron impact reactions with NS plasma. for the same input energy, thermal ignition delay is ~ 60% higher. plasma generated radicals trigger heat release from fuel oxidation at ~700 K, as opposed to autoignition temperature of ~960 K under same conditions.

21 Effect of Burst Size and Dielectric constant on Ignition ignition delay vs # pulses in burst P i = 80 torr, T i = 473 K f = 40 khz, Φ = 1.0, CPT pulser ignition delay sensitivity to eq. ratio P i = 80 torr, T i = 500 K f = 60 khz, FID pulser there is a minimum # of pulses in burst, below which no ignition is observed. ignition characteristics are highly sensitive to dielectric properties. uncertainty in the dielectric constant values should be considered during the validation process. ignition delay reduction with increase in burst size is especially pronounced for lean mixtures.

22 Effect of Pressure and Pulsing Rates on H -Air Ignition T i = 473 K, f = 40 khz, ϕ = 1.0, CPT pulser ignition delay reduction with increase in pressure is well reproduced by the model. increase in pressure results in nearly linear rise in input energy per pulse because of its dependence on number density. Faster addition of energy results in more rapid ignition at higher pressures. the nonlinear trend of # pulses required for ignition as a function of pulsing frequency is not reproduced by the model. the model predicts that input energy per pulse is nearly independent of pulsing frequency, which may not be true. lowering of input energy, because of residual electron density effects, with rise in pulsing rates may explain the observed nonlinear trend.

23 OH Density Decay after 50 Pulse Burst in CH 4 -, and C H 4 -Air Mixtures P i = 100 torr, T i = 500 K, f = 10 khz, FID pulser CH 4 -air CH 4 -air (64 species) GRI Mech 3.0 CH 4 /N /O plasma NOX reactions C H 4 -air (70 species) USC Mech C H 4 /N /O plasma NOX reactions C H 4 -air GRI Mech 3.0 has been validated extensively in K and 5 torr to 10 atm range. USC Mech has been validated in K and 16 torr to 10 atm range. model consistently over-predicts OH density by ~50% in CH 4 -air mixtures. growth rate is correctly predicted in C H 4 -air mixtures, but the decay rate in slower than measurements. low temperature uncertainty in chain reactions may be the primary reason for deviations Ongoing Work different CH 4 - and C H 4 -air combustion chemistry integrated with plasma kinetics are being tested to assess their relative performance on predicting low temperature radical production/decay.

24 Temperature 1st stage R-H R (H abstraction) R + O RO (exothermic) RO HO, H O, CH O etc. time Nanosecond Plasma Ignition of nheptane-air (in collaboration with Wenting Sun) nd stage H O OH CH O CO, H O CO CO Objective understand the effect of NS plasma on n- heptane-air ignition chemistry through self-consistent simulations. investigate the effect of radical addition to the low temperature and high temperature steps of the -stage ignition process. nc 7 H 16 -air plasma combustion kinetics (154 species) C 7 H 16 /N /O combustion (LLNL reduced mech + NOX reactions) n C H OH C H H O C H OOH C H O OH C H O CH CHO O 3 CH O OH HCO H O H O O OH H O M OH OH M e N N A B C a e (,,, ) e N N N( D) e e O O O( D) e e C H C H H e e C H C H CH e e C H C H C H e C 7 H 16 /N /O plasma reactions* N ( A ) O N O O 3 N ( A ) C H N C H H N ( A ) C H N C H H N ( A ) C H N C H CH O( D) C7H16 C7H15 OH * C 7 H 16 (electron impact and with excited species) reaction rates estimated from C 3 H 8 based plasma reactions.

25 Nanosecond Plasma Ignition of nheptane-air Effect of NS Pulses on 1st Stage Delay Time model geometry operating conditions O, H and OH density evolution at center of discharge volume P i = 160 torr T i = 600 K f = 60 khz Φ = kv Gaussian pulses 10 ns duration temperature evolution at center of discharge volume self-acceleration of low temperature chemistry application of 6 NS pulses significantly accelerates 1st stage temperature rise (by ~ 10 times) addition of small amount of radicals accelerates the H abstraction step RO produces more radicals which accelerate the whole process further. auto ignition R-H R RO CH O, HO, H O

26 Nanosecond Plasma Ignition of nheptane-air Effect of NS Pulses on Overall Ignition Delay Time operating conditions P i = 160 torr T i = 600 K f = 60 khz Φ = kv Gaussian pulses 10 ns duration only a few NS pulses sufficient to rapidly trigger 1st stage temperature rise staggered application of NS pulses NS pulser off 5 NS pulses are applied after the 1st stage to reduce the overall ignition delay time with NOX chemistry without NOX chemistry auto ignition the staggered application of NS pulses result in ~ 40% reduction in ignition delay time it is evident that the nd stage is less sensitive to radical addition by NS pulses than the 1st stage. heating provided by the NS pulses after the 1st stage accelerate the decomposition of H O and reduce ignition delay. H O + M OH + M inclusion of NOX catalytic reactions change the predictions by ~5% because of following new OH generation pathways. NO + HO NO + OH NO + CH 3 O NO + CH O + OH

27 cm physical setup Nanosecond plasma coupled premixed flame CH 4 -air operating conditions Pressure: 5 torr Inlet Temperature: 650 K Eq. ratio: 1.07 Gap width: 4.0 cm initial Electron Density: 10 7 cm kv peak voltage 7 ns FWHM Mdot : kg/m -s applied voltage validation of flame model with CHEMKIN solution CH 4 -air plasma flame kinetics (75 species) GRI Mech CH 4 /N /O /CO/CO plasma + NOX chemistry electron impact processes of both reactant (CH 4, O, N ) and product species (H O, CO, CO ) considered. N e N A B C a e (,,, ) O e O O e CO e CO* e H O e O H what are most important plasma pathways pertaining to H O, CO, CO? is plasma species production in preheat zone more important than downstream?

28 cm Plasma Coupled Premixed CH 4 -Air Flame P i = 5 torr, T i = 650 K, Φ = 1.07 physical setup reduced electric field vs height preheat zone flame zone electron density vs height high E/N ( Td) and high electron densities (~1e13 cm -3 ) allow for efficient radical generation by NS pulses in preheat zone, where they may provide significant benefit. note that radicals (O, H, OH etc) concentration in the flame zone is already of the order 10,000 ppm, so plasma cannot make much impact high E/N downstream of the flame can be attributed to high temperatures and low number density. E/N in the preheat zone reaches ~ 600 Td at.5 ns. Plasma radical generation in this zone may have a significant impact on flame characteristics. sharp peak in the E/N profile at 0 ns at the right boundary indicates the cathode sheath region. electron density distribution is fairly uniform in the entire domain reaching peak value of x10 13 cm -3 at 7.5 ns. total input energy during the pulse was.7 mj

29 cm Plasma Coupled Premixed CH 4 - Air Flame P i = 5 torr, T i = 650 K, Φ = 1.07 physical setup N excited species vs height O atom density vs height plasma generation of O atoms in the preheat zone may provide significant benefits. the production rates of N (A 3 ) and N (B 3 ) in the preheat zone is about times higher than downstream because of higher N number density. electron impact dissociation of O in the preheat zone results in ~30 times increase in O atom density within 30 ns the excited species are quenched rapidly after the pulse resulting in further production of O and other radicals ongoing work we are performing longer timescale simulations to understand the effect of repetitive application of discharge pulses on flame dynamics. the effect of NS discharges on H -air, CH 4 -air and C H 4 -air premixed flames are being investigated. close collaboration with OSU group is pursued for obtaining greater insight through experiments and high fidelity modeling

30 Where we go from here? High fidelity 1D numerical tools for construction and validation of robust plasma combustion kinetic models detailed studies of the plasma coupled premixed flame system for a variety of fuels. development of the counterflow plasma flame simulation framework. close collaboration with other MURI team members for model validation and critical assessment of the plasma combustion kinetic models D/3D simulations of nonequilibrium plasma in complex flow environments High fidelity simulations of single filament discharge in D with detailed chemistry. Large Eddy Simulation (LES) of H jet in supersonic O crossflow in the presence of a nanosecond plasma source. theoretical framework to understand plasma-flow interactions.

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